The application of layered solids for molecular recognition is summarized. By using layered solids (silicates, aluminosilicates, titanates, hydroxides, and so on), ions and molecules can be concentrated from aqueous and vapor phases. The large surface area and tunable surface properties derived from the layered structures contribute to molecular recognition. The choice of materials and modification of the nanostructure were carefully investigated to optimize the performance based on molecular recognition (selective adsorption, substrate selective reaction, detection, etc.). The progress made in materials syntheses (variation of layered materials, sophisticated modification, controlled morphology, and processing) has made the design of materials more attractive and realistic.